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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Guest Hydrogen Bond Dynamics and Interactions in the Metal-Organic Framework MIL-53(AI) Measured with Ultrafast Infrared Spectroscopy
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Guest Hydrogen Bond Dynamics and Interactions in the Metal-Organic Framework MIL-53(AI) Measured with Ultrafast Infrared Spectroscopy

机译：通过超快红外光谱测量的金属 - 有机框架MIL-53（AI）的氢键动力学和相互作用

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摘要

MIL-53(Al) is among the most "flexible" metal organic frameworks and significantly changes its structure when guest molecules are introduced into the framework's pores. The guest molecules interact with mu(2)-OH, which is a hydroxyl group bridging two aluminums. This interaction is thought to play an important role in the adsorption of molecules into the pores. Here, we report infrared absorption, infrared pump probe, and two-dimensional infrared spectroscopy on a deuterated bridging hydroxyl, mu(2)-OD, in MIL-53(Al) loaded with various guest molecules. Depending on guest, large vibrational frequency shifts, broadening of absorption band, enhancement of absorption coefficient, and acceleration of vibrational relaxation were observed, which are all signatures of hydrogen bonding interactions between the bridging hydroxyls and the guest. 2D IR spectroscopy reveals that the time evolution of the vibrational frequency occurs on multiple time scales: subpicosecond dynamics caused by localized hydrogen bond fluctuations and picosecond dynamics of the framework lattice, followed by significantly slower dynamics likely induced by global reconfigurations of the guest molecules in the pores. When benzonitrile, a strong hydrogen bonding agent, is introduced into the pores, an oscillatory feature was observed in the time evolution of the frequency, which was assigned to underdamped hydrogen bond fluctuations.
机译：MIL-53（AL）是最“柔性”的金属有机框架之一，并且当客体分子引入框架的孔隙时显着改变其结构。客体分子与Mu（2）-OH相互作用，该μOH是桥接两个铝的羟基。认为这种相互作用在将分子吸入孔隙中发挥着重要作用。在此，我们在载于各种客体分子的MIL-53（A1）中，向红外吸收，红外泵探针和二维红外光谱报告在氘代桥上的氘代桥上，MU（2）-od。根据客人，大大振动频率换档，吸收带扩大，吸收系数的增强以及振动弛豫的加速度，这是桥接羟基和客人之间的氢键相互作用。 2D IR光谱揭示了振动频率的时间演变在多个时间尺度上发生：由框架格子的局部氢键波动和PICOSecond动态引起的蛛网二十次动态，随后通过全球对客体分子的全球重新配置引起的动态显着较慢的动态毛孔。当苄腈时，将强氢键剂引入孔中时，在频率的时刻演化中观察到振荡特征，其被分配给欠扫氢键波动。

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